Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 33, Pages 7881-7887Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201806281
Keywords
hydrogels; peptide amphiphiles; self-assembly; supramolecular chemistry; thermal history
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Funding
- European Research Council under the European Union [258775]
- University of East Anglia
- European Research Council (ERC) [258775] Funding Source: European Research Council (ERC)
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The possibility of using differential pre-heating prior to supramolecular gelation to control the balance between hydrogen-bonding and aromatic stacking interactions in supramolecular gels and obtain consequent systematic regulation of structure and properties is demonstrated. Using a model aromatic peptide amphiphile, Fmoc-tyrosyl-leucine (Fmoc-YL) and a combination of fluorescence, infrared, circular dichroism and NMR spectroscopy, it is shown that the balance of these interactions can be adjusted by temporary exposure to elevated temperatures in the range 313-365 K, followed by supramolecular locking in the gel state by cooling to room temperature. Distinct regimes can be identified regarding the balance between H-bonding and aromatic stacking interactions, with a transition point at 333 K. Consequently, gels can be obtained with customizable properties, including supramolecular chirality and gel stiffness. The differential supramolecular structures also result in changes in proteolytic stability, highlighting the possibility of obtaining a range of supramolecular architectures from a single molecular structure by simply controlling the pre-assembly temperature.
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